4.4 Article

Construction of silsesquioxane and phosphinum-based ionic porous hypercrosslinked polymers for efficient heterogeneous catalytic CO2 cycloaddition

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JOURNAL OF POLYMER SCIENCE
卷 -, 期 -, 页码 -

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WILEY
DOI: 10.1002/pol.20230335

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CO2 cycloaddition; heterogeneous catalysis; ionic porous hypercrosslinked polymers; phosphinum salts; polyhedral oligomeric silsesquioxanes

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A facile method was reported to construct polyhedral oligomeric silsesquioxane (POSS) and phosphonium-based ionic porous hypercrosslinked polymers (P-iPHCPs) with multiple catalytic active sites. These polymers, with hierarchical micro/mesoporous structures and flower-like nano-morphology, serve as efficient heterogeneous catalysts for the conversion of carbon dioxide (CO2) to valuable cyclic carbonates. Particularly, polymer P-iPHCP-14 exhibits high efficiency in the synergistic catalytic conversion of CO2 with various epoxides to cyclic carbonates under mild conditions, and is recyclable.
In this work, we reported a facile one-pot route to construct polyhedral oligomeric silsesquioxane (POSS) and phosphonium-based ionic porous hypercrosslinked polymers (denoted as P-iPHCPs) with multiple catalytic active sites, which could be regarded as efficient heterogeneous catalysts for the conversion of carbon dioxide (CO2) to highly value-added cyclic carbonates. The targeted polymers P-iPHCPs were prepared from a rigid building block octavinylsilsesquioxane (VPOSS) and a low-cost commercially available organic ionic salt methyltriphenylphosphonium bromide ([Ph3PMe]Br) by the AlCl3-catalyzed Friedel-Crafts reaction. The series of polymers P-iPHCPs that synthesized by different molar ratios of VPOSS to [Ph3PMe]Br possess hierarchical micro/mesoporous structures with high surface areas ranging from 376 to 429 m(2) g(-1) and behave the flower-like nano-morphology. Especially, the desired multiple active sites involved the mixed anions including free Cl-, Br- anions and the in-situ formed metal-halogen complex anion [AlCl3Br](-) within phosphonium segments, and the enriched POSS-derived Si-OH hydrogen bond donor (HBD) groups that derived from the breakage of POSS cages during the synthetic process. The typical polymer P-iPHCP-14 has the aforementioned nucleophilic-electrophilic multiple catalytic active sites, which was regarded as an efficient recyclable heterogeneous catalyst for synergistic catalytic conversion of CO2 with various epoxides into cyclic carbonates under mild conditions.

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